The Cloud Absorption Radiometer (CAR) was flown aboard the University of Washington Convair CV-580 research aircraft during the Southern Africa Regional Science Initiative 2000 (SAFARI 2000) dry season campaign and obtained measurements of bidirectional reflectance distribution function (BRDF) for a variety of natural surfaces and ecosystems in southern Africa. To measure the BRDF of the surface–atmosphere system, the University of Washington CV-580 banked at a roll angle of ~20° and flew circles about 3 km in diameter above the surface, taking approximately 2 min. Multiple circular orbits were acquired over selected surfaces so that average BRDFs could be acquired, smoothing out small-scale surface and atmospheric inhomogeneities. In this paper, we present results of BRDFs taken over two Earth Observing System (EOS) validation sites: Skukuza tower, South Africa (25.0°S, 31.5°E) and Mongu tower, Zambia (15.4°S, 23.3°E). Additional sites are discussed and include the Maun tower, Botswana (20.0°S, 23.6°E), Sua Pan, Botswana (20.6°S, 25.9°E), Etosha Pan, Namibia (19.0°S, 16.0°E), and marine stratocumulus clouds off the west coast of Namibia (20.5°S, 13.1°E). Results clearly show anisotropy in reflected solar radiation over the various surfaces types: savanna, salt pans, and cloud. The greatest anisotropy is observed over marine stratus clouds, which exhibit strong forward scattering as well as important water cloud scattering features such as the rainbow and glory. The BRDF over savanna is characterized by a distinct backscattering peak in the principal plane and shows directional and spectral variations. Over the pans, the BRDF is more enhanced in the backscattering plane than forward scattering plane and shows little directional variation.